The physical implementation of quantum information processing relies on individual modules-qubits-and operations that modify such modules either individually or in groups-quantum gates. Two examples ...of gates that entangle pairs of qubits are the controlled NOT-gate (CNOT) gate, which flips the state of one qubit depending on the state of another, and the gate that brings a two-qubit product state into a superposition involving partially swapping the qubit states. Here we show that through supramolecular chemistry a single simple module, molecular {Cr7Ni} rings, which act as the qubits, can be assembled into structures suitable for either the CNOT or gate by choice of linker, and we characterize these structures by electron spin resonance spectroscopy. We introduce two schemes for implementing such gates with these supramolecular assemblies and perform detailed simulations, based on the measured parameters including decoherence, to demonstrate how the gates would operate.
Linking polymetallic cages can be a method for creating new structures and new properties. In this tutorial review we use heterometallic anti-ferromagnetically coupled rings (AF-rings) as exemplars ...for three approaches that can be used to link cage compounds. The first of three routes involves an ion-pair interaction supported by hydrogen-bonding interactions, which allows the synthesis of hybrid rotaxanes among other materials. The second route involves functionalising the exterior of the AF-ring so that it will act as a Lewis base; complexes involving coordination of pyridine to bridging monometallic and dimetallic fragments are discussed. The third route involves creating a vacancy on one site of the AF-ring, and then using the ring as a Lewis acid. Di-imine ligands can then be used to link the AF-rings into dimers. A brief discussion of the physical properties of these systems is also included.
A synthetic strategy is demonstrated to prepare two distinct trimers of antiferromagnetically coupled {Cr7Ni} rings, substantially varying the magnetic interactions between the spin centres. The ...interactions were studied using multi‐frequency cw EPR: in a trimer linked via non‐covalent H‐bonding interactions no measurable interaction between rings was seen, while in a trimer linked via iso‐nicotinate groups isotropic and anisotropic exchange interactions of +0.42 and −0.8 GHz, respectively, were observed. The latter are the same as those for a simpler hetero‐dimer system, showing how the spin‐spin interactions can be built in a predictable and modular manner in these systems.
Chemical coupling of antiferromagnetic rings into hetero‐spin supramolecular structures is reported by different routes: control of molecule…molecule magnetic interactions is demonstrated with transferability of parameters from simpler building blocks.
Coherent control of individual molecular spins in nanodevices is a pivotal prerequisite for fulfilling the potential promised by molecular spintronics. By applying electric field pulses during ...time-resolved electron spin resonance measurements, we measure the sensitivity of the spin in several antiferromagnetic molecular nanomagnets to external electric fields. We find a linear electric field dependence of the spin states in Cr_{7}Mn, an antiferromagnetic ring with a ground-state spin of S=1, and in a frustrated Cu_{3} triangle, both with coefficients of about 2 rad s^{-1}/V m^{-1}. Conversely, the antiferromagnetic ring Cr_{7}Ni, isomorphic with Cr_{7}Mn but with S=1/2, does not exhibit a detectable effect. We propose that the spin-electric field coupling may be used for selectively controlling individual molecules embedded in nanodevices.
An enormous family of heterometallic rings has been made. The first were Cr7M rings where M=NiII, ZnII, MnII, and rings have been made with as many as fourteen metal centers in the cyclic structure. ...They are bridged externally by carboxylates, and internally by fluorides or a penta‐deprotonated polyol. The size of the rings is controlled through templates which have included a range of ammonium or imidazolium ions, alkali metals and coordination compounds. The rings can be functionalized to act as ligands, and incorporated into hybrid organic–inorganic rotaxanes and into molecules containing up to 200 metal centers. Physical studies reported include: magnetic measurements, inelastic neutron scattering (including single crystal measurements), electron paramagnetic resonance spectroscopy (including measurements of phase memory times), NMR spectroscopy (both solution and solid state), and polarized neutron diffraction. The rings are hence ideal for understanding magnetism in elegant exchange‐coupled systems.
A playground for physics: Heterometallic rings featuring seven trivalent and a single divalent metal center were first reported in 2003. Since that time they have been shown to be ideal for studying the physics of anti‐ferromagnetically coupled nanomagnets. They have a rich chemistry, and can be incorporated in larger structures in at least three ways, including use of the inorganic rings as part of hybrid rotaxanes.
Quantum information processing (QIP) would require that the individual units involved--qubits--communicate to other qubits while retaining their identity. In many ways this resembles the way ...supramolecular chemistry brings together individual molecules into interlocked structures, where the assembly has one identity but where the individual components are still recognizable. Here a fully modular supramolecular strategy has been to link hybrid organic-inorganic 2- and 3-rotaxanes into still larger 4-, 5- and 7-rotaxanes. The ring components are heterometallic octanuclear Cr7NiF8(O2C(t)Bu)16(-) coordination cages and the thread components template the formation of the ring about the organic axle, and are further functionalized to act as a ligand, which leads to large supramolecular arrays of these heterometallic rings. As the rings have been proposed as qubits for QIP, the strategy provides a possible route towards scalable molecular electron spin devices for QIP. Double electron-electron resonance experiments demonstrate inter-qubit interactions suitable for mediating two-qubit quantum logic gates.
Field-emission devices are promising candidates to replace silicon fin field-effect transistors as next-generation nanoelectronic components. For these devices to be adopted, nanoscale field emitters ...with nanoscale gaps between them need to be fabricated, requiring the transfer of, for example, sub-10 nm patterns with a sub-20 nm pitch to substrates like silicon and tungsten. New resist materials must therefore be developed that exhibit the properties of sub-10 nm resolution and high dry etch resistance. A negative tone, metal–organic resist is presented here. It can be patterned to produce sub-10 nm features when exposed to helium ion beam lithography at line doses on the order of tens of picocoulombs per centimeter. The resist was used to create 5 nm wide, continuous, discrete lines spaced on a 16 nm pitch in silicon and 6 nm wide lines on an 18 nm pitch in tungsten, with line edge roughness of 3 nm. After the lithographic exposure, the resist demonstrates high resistance to silicon and tungsten dry etch conditions (SF6 and C4F8 plasma), allowing the pattern to be transferred to the underlying substrates. The resist’s etch selectivity for silicon and tungsten was measured to be 6.2:1 and 5.6:1, respectively; this allowed 3 to 4 nm thick resist films to yield structures that were 21 and 19 nm tall, respectively, while both maintained a sub-10 nm width on a sub-20 nm pitch.
The tetravalency of carbon and its ability to form covalent bonds with itself and other elements enables large organic molecules with complex structures, functions and dynamics to be constructed. The ...varied electronic configurations and bonding patterns of inorganic elements, on the other hand, can impart diverse electronic, magnetic, catalytic and other useful properties to molecular-level structures. Some hybrid organic-inorganic materials that combine features of both chemistries have been developed, most notably metal-organic frameworks, dense and extended organic-inorganic frameworks and coordination polymers. Metal ions have also been incorporated into molecules that contain interlocked subunits, such as rotaxanes and catenanes, and structures in which many inorganic clusters encircle polymer chains have been described. Here we report the synthesis of a series of discrete rotaxane molecules in which inorganic and organic structural units are linked together mechanically at the molecular level. Structural units (dialkyammonium groups) in dumb-bell-shaped organic molecules template the assembly of essentially inorganic 'rings' about 'axles' to form rotaxanes consisting of various numbers of rings and axles. One of the rotaxanes behaves as a 'molecular shuttle': the ring moves between two binding sites on the axle in a large-amplitude motion typical of some synthetic molecular machine systems. The architecture of the rotaxanes ensures that the electronic, magnetic and paramagnetic characteristics of the inorganic rings-properties that could make them suitable as qubits for quantum computers-can influence, and potentially be influenced by, the organic portion of the molecule.
Celotno besedilo
Dostopno za:
DOBA, IJS, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
We report a supramolecule that contains five spins of two different types and with, crucially, two different and predictable interaction energies between the spins. The supramolecule is ...characterized, and the interaction energies are demonstrated by electron paramagnetic resonance (EPR) spectroscopy. Based on the measured parameters, we propose experiments that would allow this designed supramolecule to be used to simulate quantum decoherence in maximally entangled Bell states that could be used in quantum teleportation.
Molecules that are the size of small proteins are difficult to make. The most frequently examined route is via self-assembly, and one particular approach involves molecular nanocapsules, where ...ligands are designed that will enforce the formation of specific polyhedra of metals within the core of the structure. Here we show that this approach can be combined with mechanically interlocking molecules to produce nanocapsules that are decorated on their exterior. This could be a general route to very large molecules, and is exemplified here by the synthesis and structural characterization of a 13rotaxane, containing 150 metal centres. Small angle X-ray scattering combined with atomistic molecular dynamics simulations demonstrate the compound is intact in solution.
PDF
